KR20230132791A - Membrane attachment technology - Google Patents

Abstract

1. A method of securing a membrane to a substrate, the method comprising: depositing a metal layer on the surface of the substrate; and performing a bonding process to bond a metal membrane to the deposited metal layer.

Description

Membrane attachment technology

The field of the invention relates to the provision of membrane arrangements. Aspects provide improved techniques for securing a metal membrane to a substrate.

Hydrogen is increasingly used as an energy source. The advantage of hydrogen is that it is a clean fuel in that it burns to produce water. Applications where hydrogen can be used as a combustible fuel include powering ships and providing domestic gas. Hydrogen can also be used in fuel cells as an environmentally friendly alternative to conventional batteries.

An efficient form of hydrogen production is production from syngas. Synthetic gas can be produced by reforming natural gas. Syngas is a gas mixture containing primarily carbon monoxide and/or carbon dioxide, and hydrogen. Syngas may also contain amounts of other gases, such as carbon dioxide and methane. A water gas shift reaction can be performed on the synthesis gas to increase the concentration of hydrogen in the gas mixture. To produce substantially pure hydrogen, the hydrogen must be separated from other gases in the gas mixture.

A known technique for separating hydrogen from other gases is to use palladium alloy membranes. The gas mixture passes through a pipe where the membrane is the pipe wall. Hydrogen diffuses through the membrane and is thereby separated from other gases in the gas mixture that cannot pass through the membrane.

In known hydrogen separators the membrane thickness is generally on the order of 100 micrometers. The rate at which hydrogen can pass through the membrane is inversely proportional to the membrane thickness and proportional to the membrane surface area. Separation of hydrogen by these membranes is slow due to the large membrane thickness. Additionally, palladium is expensive, so implementation costs are high.

There is a general need to improve known gas separation devices, especially known membrane attachment technologies.

SUMMARY OF THE INVENTION

According to a first aspect of the invention, there is provided a method of securing a membrane to a substrate, the method comprising: depositing a metal layer on the surface of the substrate; and performing a bonding process to bond the metal membrane on the deposited metal layer.

Preferably, the deposited metal layer includes silver, palladium, nickel and/or copper.

Preferably, the deposited metal layer has a thickness of 0.01 to 1 micrometer, preferably 0.01 to 0.50 micrometer, more preferably about 0.1 micrometer or about 0.5 micrometer.

Preferably, the metal membrane comprises palladium and/or a palladium alloy.

Preferably, depositing the metal layer includes performing a sputtering process.

Preferably, the bonding process lasts from about 1 minute to about 350 hours, preferably from about 10 minutes to about 24 hours, more preferably from about 1 hour to about 12 hours, so that the bonding process lasts about 1 hour, more preferably. Typically, it should last for about 6 to 8 hours.

Preferably, the bonding process includes applying heat and pressure in a closed environment.

Preferably, the pressure applied in the bonding process is 1 to 30 barg, preferably 5 to 20 barg, and more preferably 5 barg.

Preferably, the applied pressure is gas pressure.

Preferably, the applied pressure is a mechanically applied pressure.

Preferably, the sealed environment contains hydrogen gas.

Preferably, the sealed environment contains 10 to 80% by volume of hydrogen gas, preferably 20 to 70% by volume of hydrogen gas, more preferably 40% by volume.

Preferably, the sealed environment contains substantially only inert gases, such as nitrogen gas.

Preferably, the deposited metal layer comprises palladium; The temperature applied in the bonding process is 200°C to 500°C, preferably 400°C to 450°C.

Preferably, the deposited metal layer comprises copper, silver or nickel; The temperature applied in the bonding process is 350°C to 450°C, preferably about 440°C.

Preferably, the metal membrane includes one or more metals other than palladium.

Preferably, the metal membrane comprises silver; Preferably, the metal membrane is 15% to 40% by weight silver and substantially the remainder of the metal membrane is palladium; More preferably, the metal membrane is about 77% palladium and about 23% silver by weight.

Preferably, the thickness of the metal membrane is less than 10 micrometers, preferably 0.2 to 5 micrometers, more preferably 1 to 4 micrometers.

According to a second aspect of the invention, there is provided a membrane arrangement comprising a metal membrane secured to a substrate, wherein the membrane arrangement is manufactured according to the method of the first aspect.

Preferably, the membrane arrangement is for separating the first gas from one or more other gases in the gas separation device.

Preferably, the first gas is hydrogen and one or more other gases include nitrogen, methane, carbon monoxide and/or carbon dioxide.

According to a third aspect of the invention, there is provided a gas separation section for separating a first gas from one or more other gases in the separation device, the gas separation section having: a substantially planar second side; a first membrane arrangement according to; comprising a second membrane arrangement along the second side that is substantially planar; The substrate of the first membrane arrangement has a first surface and a second surface, the second surface being opposite the substrate of the first membrane arrangement than the first surface of the substrate of the first membrane arrangement; The substrate of the second membrane arrangement has a first surface and a second surface, the second surface being opposite the substrate of the second membrane arrangement than the first surface of the substrate of the second membrane arrangement; The gas separation portion includes a mesh arranged between the second surface of the substrate of the first membrane arrangement and the second surface of the substrate of the second membrane arrangement; The membrane of the first membrane arrangement is secured to the first surface of the first membrane arrangement; the membrane of the second membrane arrangement is secured to the first surface of the substrate of the second membrane arrangement.

According to a fourth aspect of the invention, there is provided a separation device for separating a first gas from one or more other gases, the separation device comprising: an inlet for receiving a gas mixture comprising the first gas and the one or more other gases. (inlet); A plurality of gas separation units according to a third aspect, comprising: a plurality of gas separation units arranged in a stack; a first outlet arranged to output a first gas that has passed through one or more of the membranes within the one or more gas separators; and a second outlet arranged to exhaust at least one other gas that has not passed through one or more of the membranes within the one or more gas separators.

According to a fifth aspect of the invention, there is provided a method for separating a first gas from a gas mixture comprising the first gas and at least one other gas, the method comprising supplying the gas mixture to the separation device according to the fourth aspect. step; receiving a first gas stream comprising substantially only a first gas from the separation device; and receiving a second gas flow comprising at least one gas other than the first gas from the separation device.

The accompanying drawings, which are incorporated into this specification and form part of the description, illustrate aspects of the invention and serve to clarify some aspects of the invention and to enable those skilled in the art(s) to make and use aspects of the invention. let it be
1A, 1B and 1C illustrate steps in a process for securing a membrane to a substrate according to embodiments;
Figure 2 shows a membrane arrangement according to an embodiment;
3 is a cross-sectional view of some components of a separation device that may include a membrane arrangement according to an embodiment;
4A and 4B illustrate gas separation that may include a membrane arrangement according to embodiments;
4C shows a stack of gas separation units that may include a membrane arrangement according to an embodiment;
5 shows a portion of a separation device that may include a membrane arrangement according to an embodiment;
6 is a flow diagram of a method according to an aspect.

WO 2020/012018 A1, the entire content of which is incorporated herein by reference, discloses a gas separation device that advantageously provides a large membrane surface area with a low membrane thickness. In a gas separation device, a plurality of membranes are attached to each of a plurality of substrates to separate hydrogen. However, attaching thin membranes to substrates presents many technical challenges. When using known techniques for attaching thin membranes to substrates, problems that may be encountered include, for example, leakage and/or separation of the membrane. These problems increase the manufacturing cost and reliability of the gas separation device.

Aspects provide improved techniques for securing a membrane to a substrate. This aspect is particularly suitable for attaching thin membranes to substrates. A preferred application of the embodiment is in the construction of a membrane arrangement for use in a gas separation device as disclosed in WO 2020/012018 A1.

1A, 1B, and 1C show steps in a membrane attachment technique according to embodiments.

The membrane attachment technique according to the embodiment makes it possible to attach a membrane 103 , which may be a thin membrane 103 , to a substrate 101 . Advantages of the embodiment over known techniques include more secure attachment of the membrane 103 to the substrate 101, reduced risk of gas leakage around the attached membrane, and lower risk of separation of the membrane 103 from the substrate 101. , and increasing membrane life.

Membrane 103 may be a palladium membrane. Figure 1a shows the substrate 101 on which the palladium membrane 103 is to be fixed. The substrate 101 may be made of metal, ceramic, polymer, or a combination thereof. Preferably, the substrate 101 is a sintered plate. Preferably, the substrate 101 is made of AISI316L.

The substrate 101 according to aspects may have properties that allow hydrogen to pass through. The substrate 101 is a porous material, or a material permeable to hydrogen due to solid diffusion (e.g. electron and oxygen ion conducting and/or proton conducting ceramics or mixed conductors of metals of groups IVB and VB), or a material thereof. It may be a layered combination.

Inventors realized that palladium, as a material property, had the potential to grow on its own as well as other materials. This is used in aspects to improve the adhesion of the palladium membrane 103 to the substrate 101.

In Figure 1B, a very thin metal layer 102, which may include palladium, is first deposited on the surface of the substrate 101. The metal layer 102 may be deposited on the substrate through sputtering deposition. The sputtering deposition process can be performed in a practical vacuum. Alternatively, metal layer 102 may be deposited on the substrate by any other known deposition technique.

The effect of the deposited metal layer 102 may be that the surface peaks on the surface of the substrate 101 are covered with the deposited metal, in this embodiment comprising palladium. The amount of metal deposited may be the amount necessary to substantially cover the surface peaks. The metal layer 102 covering the surface peak may have a thickness of, for example, 0.01 to 1 micrometer, more preferably 0.03 to 0.3 micrometer, more preferably 0.1 to 0.25 micrometer, and more preferably has a thickness of It's about 0.1 micrometer.

In Figure 1C, the palladium membrane 103 is placed on the deposited metal layer 102 and the palladium membrane 103 is bonded to the deposited metal layer 102 by a bonding process, which is a burn-in process. ) can be referred to as. The burn-in process may cause the membrane 103 to grow into the deposited metal layer 102 on the substrate 101. This allows the membrane 103 to grow into surface peaks on the surface of the substrate 101 and, as a result, to be fixed to the substrate 101 . Embodiments also include a palladium alloy membrane 103 similarly disposed on a deposited metal layer 102 and a palladium alloy membrane 103 similarly bonded to the deposited metal layer 102 by a bonding process.

Membrane 103 according to aspects may be less than 10 micrometers thick. That is, at a distance perpendicular to the plane of the membrane 103, the planar major surfaces of the membrane 103 are less than 10 micrometers apart from each other. Membrane 103 is preferably 0.2 to 5 micrometers thick, more preferably 1 to 4 micrometers thick.

Membrane 103 according to embodiments may be comprised substantially entirely of palladium. Alternatively, membrane 103 may include one or more palladium and metals other than palladium.

The composition of the membrane 103 is preferably such that 15% to 40% of the weight is silver and the remaining weight is palladium. Preferably, the composition of the membrane 103 is such that 1/5 to 1/3 of its weight is silver and the remainder is palladium. More preferably, the composition of the membrane 103 is 77% by weight palladium and 23% by weight silver.

Membrane 103 may include palladium, silver, and metal X and/or metal Y, where metal X is different from metal Y, and metal X and metal Y are both metals other than palladium and silver.

The most appropriate conditions for the burn-in process for bonding the membrane 103 to the deposited metal layer 102 may vary depending on both the composition of the deposited metal layer 102 and the composition of the membrane 103.

Suitable conditions for the burn-in process are described below according to the first aspect. In a first aspect, deposited metal layer 102 is palladium or includes palladium and membrane 103 is palladium or includes palladium.

The burn-in process may last for up to about 350 hours, preferably the burn-in process lasts for up to about 14 days, preferably the burn-in process lasts for less than about 24 hours, more preferably The burn-in process lasts for about 1 to about 12 hours, preferably the burn-in process lasts for about 6 to about 8 hours. The burn-in process can last for approximately 1 hour. The burn-in process may last from about 1 minute to about 350 hours, or from about 10 minutes to about 24 hours, or from about 30 minutes to about 1 hour.

The burn-in process may include applying heat and pressure in a sealed environment. The burn-in process is preferably carried out at up to about 650°C or higher, preferably at about 200°C to 500°C, preferably at about 300°C to 450°C, more preferably at about 380°C to about 480°C, more preferably Typically on the low end, between about 400°C and 450°C. The burn-in process is preferably performed at a pressure of about 1 to about 30 barg, preferably about 5 to about 20 barg, more preferably 5 barg. The process time of the burn-in process may be correlated to the applied temperature. For example, if the applied temperature is higher, a shorter process time may be sufficient. The pressure applied in the burn-in process may be the applied gas pressure. The pressure applied may alternatively be a mechanically applied pressure. A piston (or other device/surface) may press against the membrane to exert pressure, for example. For example, a piston can exert a pressure of approximately 2000 kN/m ² .

The burn-in process can be performed in a closed environment containing hydrogen gas. The sealed environment may contain from about 10 to about 80 vol. % hydrogen gas (so there may be 70 vol. % hydrogen gas), preferably from about 20 to about 70 vol. % hydrogen gas, and more preferably may contain about 40% by volume of hydrogen gas. In a sealed environment, the remaining gas may be an inert gas, preferably nitrogen gas, but may be another inert gas such as argon.

In a second aspect of the burn-in process, the burn-in process may alternatively be performed in a closed environment that does not contain hydrogen gas. The sealed environment may contain only inert gases such as nitrogen or argon. The second aspect of the burn-in process may be performed at a higher temperature than the first aspect of the burn-in process. For example, the second aspect of the burn-in process may preferably be carried out at temperatures of up to about 650°C.

Using hydrogen in a sealed environment can improve bonding between the substrate 101 and the membrane 103. However, the advantage of using only inert gas in a sealed environment is that it may be safer to heat the substrate 101 and membrane 103 in the oven.

The burn-in process can ensure a more secure attachment of the membrane 103 to the substrate 101 than is achieved when known techniques are used. Accordingly, depending on the embodiment, a membrane arrangement comprising a membrane attached to a substrate may be more robust than a membrane arrangement manufactured according to known techniques.

Although embodiments of membrane attachment techniques have been described above with respect to palladium membranes 103, embodiments also include membranes 103 substantially comprising other metals other than palladium. For example, the aspect may be used to attach aluminum membrane 103 to a substrate.

Although embodiments of the membrane attachment technique have been described above with respect to the deposited metal layer 102 being palladium or comprising palladium, the deposited metal layer 102 may also contain other metals such as silver, copper and/or nickel instead of or in addition to palladium. May contain metal. This is because palladium can grow into substances other than itself. In particular, palladium can be grown with silver, copper, nickel, other metals and their alloys. Accordingly, the deposited metal layer 102 may include the same metal(s) and/or a different metal(s) as the membrane 103. For example, in an embodiment the deposited metal layer 102 may be silver, copper and/or nickel and the membrane 103 may be palladium. Embodiments also include a non-palladium membrane (103) and a deposited metal layer (102) that does not include palladium.

According to another embodiment, deposited metal layer 102 is copper or includes copper and membrane 103 is palladium or includes palladium. In this aspect, the thickness of the deposited metal layer 102 may range from about 0.01 to 1 micrometer, preferably about 0.25 micrometer, and more preferably about 0.1 micrometer. The appropriate temperature for the burn-in process of this embodiment is in the range of 350°C to 450°C, preferably 440°C, more preferably 400°C. The duration of the burn-in process of this embodiment can be up to 24 hours, and is preferably 6 to 8 hours. The pressure of the burn-in process of this embodiment may be about 5 to 20 barg, and is preferably 5 barg. The burn-in process can be performed in a sealed environment containing substantially only an inert gas such as nitrogen gas or argon gas.

According to another embodiment, the deposited metal layer 102 is silver or includes silver and the membrane 103 is palladium or includes palladium. In this aspect, the thickness of the deposited metal layer 102 may range from about 0.01 to 1 micrometer, preferably about 0.25 micrometer, and more preferably about 0.1 micrometer. The conditions of the burn-in process in this aspect may be as described above when the deposited metal layer 102 is copper or includes copper. Alternatively, the conditions of this aspect may be different such that a lower burn-in temperature is used.

According to another embodiment, the deposited metal layer 102 is or includes nickel and the membrane 103 is or includes palladium. In this aspect, the thickness of the deposited metal layer 102 may range from about 0.01 to 1 micrometer, preferably about 0.25 micrometer, and more preferably about 0.1 micrometer. The conditions of the burn-in process in this aspect may be as described above when the deposited metal layer 102 is copper or includes copper. Alternatively, the conditions of this aspect may be different such that a lower burn-in temperature is used.

Figure 2 shows a membrane arrangement 200 according to an embodiment. Membrane arrangement 200 includes a substrate 101 and a membrane 103 secured to the substrate 101 by the membrane attachment technique described above with respect to FIG. 1 .

Membrane arrangement 200 according to aspects may be used to separate one or more gases from a gas mixture. The membrane 103 has the property that at least one gas can pass through it, while at least one other gas in the gas mixture cannot pass through it.

The membrane attachment technology according to the aspect enables secure attachment of the thin membrane 103 to the substrate 101, so that the membrane arrangement 200 according to the aspect is reliable and leak-free in preventing gases from passing through the membrane 103. Can support high delivery rates.

In one aspect, membrane arrangement 200 can be used to separate hydrogen gas from synthesis gas. Since the water-gas shift reaction may have been carried out on synthesis gas, reference to synthesis gas should be understood as any gas mixture comprising hydrogen and one or more of other gases such as carbon monoxide, carbon dioxide, steam and methane. Embodiments include a gas mixture that is substantially a mixture of carbon dioxide and hydrogen only.

Membrane arrangement 200 comprising a palladium membrane may be particularly suitable for separating hydrogen gas from synthesis gas. Accordingly, it is possible to separate hydrogen from a mixture of hydrogen and carbon monoxide and/or carbon dioxide. Membrane arrangement 200 comprising a palladium membrane may be used more generally to separate hydrogen gas from any mixture of hydrogen gas and other gases. For example, membrane arrangement 200 comprising a palladium membrane can be used to separate hydrogen from a mixture of hydrogen and methane, a mixture of hydrogen and carbon dioxide, or a mixture of hydrogen and nitrogen.

Membrane arrangements comprising membranes other than palladium membranes may be particularly suitable for separating hydrogen and other gases from gas mixtures. Thus the embodiment can be used to separate any one or more gases that can flow through the membrane from a gas mixture.

An embodiment has been described as a membrane arrangement (200) comprising a planar membrane (103) secured on a planar surface of a substrate (101). Although this is a preferred implementation of the aspect, the aspect also includes a membrane arrangement 200 having a tubular membrane 103 secured on a tubular surface of the substrate 101. Membrane arrangement 200 may have a tubular or cylindrical structure but is otherwise substantially as described above for planar membranes.

The membrane arrangement 200 may have any suitable shape, for example a square plan, a circular plan, an annular plan, or a rectangular plan.

In the membrane arrangement 200 according to aspects, the membrane 103 is bonded directly to the substrate 101 through a burn-in process with the deposited metal layer 102. This minimizes the transport distance and transport resistance of hydrogen (or other gases to be separated) when passing through the membrane. Therefore, the gas transfer rate and therefore the gas separation rate can be increased.

Figure 3 is a cross-sectional view of part of a separation device 500 as disclosed in WO 2020/012018 A1, which is incorporated herein by reference in its entirety. Separation device 500 may include a membrane arrangement in which the membrane is secured to a substrate according to the above-described aspects of the technology.

Separation device 500 of FIG. 3 will be described in the example application of hydrogen separation from synthesis gas. As shown by the text of the large arrow in Figure 3, the embodiment includes an input gas mixture that is substantially a mixture of carbon dioxide and hydrogen only. The first emission may be substantially a stream of carbon dioxide only. The second effluent, separate from the first effluent, may be substantially a stream of hydrogen only.

Separation device 500 includes a plurality of first channels 302 and a plurality of second channels 304. Each first channel 302 is formed between a planar membrane 103, which is the wall of the first channel 302. One or more planar membranes 103 are secured to each substrate 101 according to the membrane attachment technique described with respect to FIGS. 1A-1C. Accordingly, one or more pairs of planar membranes 102 and each substrate 101 form a membrane arrangement 200 according to an aspect.

Each substrate 101 is formed from the membrane 103 on a steel mesh on the other side of the substrate 101. A mesh is provided within each of the plurality of second channels 304. Hydrogen can pass through the membrane 103, through the substrate 101 and along each second channel 304 because the mesh structure includes a gas flow path for the hydrogen. The gas input to each first channel 302 is synthetic gas. The gas discharged from each first channel 302 is referred to herein as retentate gas. The residual gas is the remaining content of the synthesis gas input to the first channel 302 after some or all of the hydrogen in the input synthesis gas passes through the membrane 103. The exhaust gas from the second channel 304 contains hydrogen that has passed through the membrane 103. Each first channel 302 has an inlet 305 for syngas at one end of the channel and an outlet 306 for retentate at the other end of the first channel 302.

At least one end of each second channel 304 is an outlet 307 for hydrogen. The embodiment also includes more than one end of the second channel 304 that is an outlet for hydrogen. In use, syngas is provided to the inlet of one or more first channels 302 and passes through each of these first channels 302 toward the outlet of each first channel 302. As the synthesis gas passes through each first channel 302, the hydrogen in the synthesis gas passes through the planar membrane 103 wall of the channel. The residual gas passing the outlet of each first channel 302 has a lower hydrogen concentration than the synthesis gas at the inlet of the first channel 302 due to hydrogen passing through the membrane 103. Preferably, the gas passing through the outlet of each first channel 302 is substantially free of hydrogen. Hydrogen passing through the membrane 103 passes through the substrate 101 into one of the second channels 304 and out of the outlet 307 of the second channel 304.

As previously described, one or more pairs of membranes and respective substrates in the gas separation device of FIG. 3 may be a membrane arrangement 200 according to an aspect. This reduces the risk of leakage of the membrane array and increases the lifespan of the membrane array by reducing the risk of the membrane detaching from the substrate.

It should be understood that the membrane arrangement 200 according to the embodiment may be used in a gas separation device having a structure different from the separation device 500 of FIG. 3. Membrane arrangements according to aspects may be used in gas separation devices that include only one first channel (302) and/or only one second channel (304). Membrane arrangements according to aspects may be used in gas separation devices that do not include mesh 304.

4a and 4b show part of an implementation of a single gas separation part 400 of a separation device 500 as disclosed in WO 2020/012018 A1. As shown in FIGS. 4A and 4B, gas separator 400 provides part of the structure as previously described with reference to FIG. 3. Each gas separator 400 includes two planar membranes 103 and each planar membrane 103 is provided on a side of the substrate 101 . One or more membranes 103 are attached to each substrate 101 by a membrane attachment technique according to aspects to form a membrane arrangement 200 . The other side of each substrate 101 is connected with a steel mesh. The mesh defines a second channel 304 between the membranes 103 to collect hydrogen.

Each gas separation unit 300 may include a hydrogen frame 401. Hydrogen frame 401 provides structural support for the mesh. The mesh supports the membrane arrangement 200.

As shown in FIGS. 4A and 4B, a gasket 303 may be provided. Gasket 303 may be a gas seal. A gasket 303 is provided to cover all edges of each membrane 103 to allow gas in the first channel 302 to flow around the end of the membrane 103 into the second channel 304 or thereabouts. Prevents reverse flow. Therefore, the only gas flow between the first channel 302 and the second channel 304 is through the membrane 103 and not around the edges of the membrane 103.

Figure 4c shows two gas separators 400 stacked one on top of the other.

A gas tight seal, for example a polymeric seal/rubber seal, may be provided to prevent any unwanted gas flow paths between adjacent gas separators 400. there is.

5 shows a portion of a gas separation device 500 according to an aspect. The separation device 500 according to the aspect preferably includes a plurality of gas separation units 400.

The segment shaped holes of the plurality of gas separation units 400 may be aligned to form four inlet/outflow channels 501, 502, 503, and 504 through stacking of the gas separation units 400. . Each inlet/outlet channel 501 , 502 , 503 , 504 may be in fluid communication with at least one input or outlet port of separation device 500 . The inlet/outlet channels can therefore provide flow paths for input syngas, outlet hydrogen and outlet residual gas.

For example, channel 502 may be an inlet channel that provides a flow path for synthesis gas from an input port for synthesis gas. The synthesis gas may flow into and along the channels 502 and into any of the gas separators 400 in a direction perpendicular to the plane of each gas separator 400 . Channel 503 may be an outlet channel that provides a flow path for residual gas to an exhaust port for residual gas. The residual gas flows from each first channel 302 to the channel 503 and then flows along the channel 503 to the discharge port in a direction perpendicular to the plane of each gas separation portion 400.

One or both of channels 501 and 504 may be a hydrogen outlet channel that provides a flow path for hydrogen to one or more outlets for hydrogen. Hydrogen may flow from each second channel 304 into at least one or both of channels 501 and 504 and then in a direction perpendicular to the plane of each gas separator 400, channels 501 and 504 ), and to at least one outlet port for hydrogen.

6 is a flow diagram illustrating a method according to aspects. At step 601, the method begins. At step 603, a metal layer is deposited on the surface of the substrate. In step 605, a bonding process is performed to bond the metal membrane onto the deposited metal layer. At step 607, the method ends.

Although the present invention has been described with respect to specific exemplary embodiments, it should be understood that various modifications, substitutions and changes may be made to the disclosed aspects without departing from the spirit and scope of the invention as set forth in the appended claims. .

Claims (23)

In the process of forming a single layer membrane structure for separating a first gas from one or more other gases in a gas separation device, a method of securing the membrane to a substrate, comprising:
Depositing a metal layer on the surface of the substrate; and
Performing a bonding process to bond a metal membrane on the deposited metal layer;
Method, including.
The method of claim 1 , wherein the deposited metal layer includes palladium, silver, nickel, and/or copper.
3. The method of claim 1 or 2, wherein the deposited metal layer has a thickness of 0.01 to 1 micrometer, preferably 0.01 to 0.50 micrometer, more preferably about 0.1 micrometer or about 0.5 micrometer. method.
4. The method according to any one of claims 1 to 3, wherein the metal membrane comprises palladium and/or a palladium alloy.
The method of any one of claims 1 to 4, wherein depositing the metal layer includes performing a sputtering process.
6. The method of any one of claims 1 to 5, wherein the bonding process lasts from about 1 minute to about 350 hours, preferably from about 10 minutes to about 24 hours, more preferably from about 1 hour to about 12 hours. Thus, the bonding process can last for about 1 hour, more preferably about 6 hours to about 8 hours.
7. The method of any one of claims 1 to 6, wherein the bonding process includes applying heat and pressure in a closed environment.
The method according to claim 7, wherein the pressure applied in the bonding process is 1 to 30 barg, preferably 5 to 20 barg, and more preferably 5 barg.
9. The method according to claim 7 or 8, wherein the applied pressure is gas pressure.
The method according to claim 7 or 8, wherein the applied pressure is mechanically applied pressure.
11. The method of any one of claims 7-10, wherein the sealed environment comprises hydrogen gas.
12. The method of claim 11, wherein the sealed environment comprises 10 to 80 vol. % hydrogen gas, preferably 20 to 70 vol. % hydrogen gas, more preferably 40 vol. % hydrogen gas.
11. The method of any one of claims 7-10, wherein the sealed environment contains substantially only an inert gas, such as nitrogen gas.
According to any one of claims 7 to 13,
The deposited metal layer includes palladium;
The method wherein the temperature applied in the bonding process is 200°C to 500°C, preferably 400°C to 450°C.
According to any one of claims 7 to 13,
The deposited metal layer includes copper, silver or nickel;
The method wherein the temperature applied in the bonding process is 350°C to 450°C, preferably about 440°C.
16. The method of any one of claims 1 to 15, wherein the metal membrane includes one or more metals other than palladium.
17. The metal membrane of claim 16, wherein the metal membrane comprises silver;
Preferably, the metal membrane is 15% to 40% silver by weight and substantially the remainder of the metal membrane is palladium;
More preferably, the metal membrane is about 77% palladium and about 23% silver by weight.
18. The method according to any one of claims 1 to 17, wherein the metal membrane has a thickness of less than 10 micrometers, preferably between 0.2 and 5 micrometers, more preferably between 1 and 4 micrometers.
A membrane arrangement comprising a metal membrane secured to a substrate,
wherein the metal membrane is comprised by a single layer membrane structure for separating a first gas from one or more other gases within a gas separation device,
A membrane arrangement, wherein the production of the membrane arrangement comprises the method according to any one of claims 1 to 18.
20. The membrane arrangement of claim 19, wherein the first gas is hydrogen and the one or more other gases include nitrogen, methane, carbon monoxide and/or carbon dioxide.
A gas separation section for separating a first gas from one or more other gases in a gas separation device, the gas separation section comprising:
A first membrane arrangement according to claim 19 or 20, which is substantially planar;
a second membrane arrangement according to claim 19 or 20, which is substantially planar;
The substrate of the first membrane arrangement has a first surface and a second surface, wherein the second surface is opposite the substrate of the first membrane arrangement than the first surface of the substrate of the first membrane arrangement. ;
The substrate of the second membrane arrangement has a first surface and a second surface, wherein the second surface is opposite the substrate of the second membrane arrangement than the first surface of the substrate of the second membrane arrangement. ;
the gas separation portion comprises a mesh arranged between a second surface of the substrate of the first membrane arrangement and a second surface of the substrate of the second membrane arrangement;
At this time, the membrane of the first membrane arrangement is fixed to the first surface of the substrate of the first membrane arrangement;
The gas separator, wherein the membrane of the second membrane arrangement is fixed to the first surface of the substrate of the second membrane arrangement.
A separation device for separating a first gas from one or more other gases, the separation device comprising:
an inlet for receiving a gas mixture comprising a first gas and one or more other gases;
A plurality of gas separation units according to claim 21, wherein the plurality of gas separation units are arranged in a stack;
a first outlet arranged to output a first gas that has passed through one or more of the membranes within the one or more gas separators; and
a second outlet arranged to exhaust at least one other gas that has not passed through one or more of the membranes within the one or more gas separation portions;
Including a separation device.
A method of separating a first gas from a gas mixture comprising the first gas and one or more other gases, the method comprising:
supplying the gas mixture to the separation device according to claim 22;
receiving a first gas stream comprising substantially only a first gas from the separation device; and
Receiving a second gas flow containing at least one gas other than the first gas from the separation device.

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